Molecular Beam Epitaxy Research Articles

Plasmonic-Metal Nanostructures-Enhanced Photoconductive Terahertz Emission and Detection

Photoconductive antennas based on low-temperature gallium arsenide (LT-GaAs) with a gold plasmonic-gold grating made of nanorods and nanoislands have been developed and fabricated. The antennas were produced using molecular beam epitaxy and electron-beam nanolithography. LT-GaAs samples with a high annealing temperature of 943 K were employed in the fabrication process. It has been demonstrated that plasmonic nanostructures significantly enhance the efficiency of light-to-terahertz radiation conversion by photoconductive antennas.

Determining the oxidation stability of SnSe under atmospheric exposure

AbstractUnderstanding surface stability becomes critical as 2D materials like SnSe are developed for piezoelectric and optical applications. SnSe thin films deposited by molecular beam epitaxy showed no structural changes after a two-year exposure to atmosphere, as confirmed by X-ray diffraction and Raman spectroscopy. X-ray photoelectron spectroscopy and reflectivity show a stable 3.5 nm surface oxide layer, indicating a self-arresting oxidative process. Resistivity measurements show an electrical response dominated by SnSe post-exposure. This work shows that SnSe films can be used in ambient conditions with minimal risk of long-term degradation, which is critical for the development of piezoelectric or photovoltaic devices. Graphical Abstract

Dodecagonal GaN Microrods: Chemical Stability of a‐, m‐, and c‐Plane Walls and Their Application to Water‐Splitting

AbstractPhotoelectrolysis of water is a sustainable option for the production of hydrogen fuel. GaN nano‐ or microstructures are considered for water‐splitting due to their general high chemical stability and high surface‐to‐volume ratio enhancing the process effectiveness. In this study GaN structures with dodecagonal microrods are used as a working electrode for the water‐splitting process. Microrods are grown using a plasma‐assisted molecular beam epitaxy process allowing tailoring of microrod height and density. Their unique property is the of presence twelve sidewalls with alternating a‐ and m‐plane orientations. This enables a simultaneous study of the chemical stability of c‐, a‐, and m‐plane walls of GaN. The water‐splitting process is performed using a 1 mol l−1 NaOH electrolyte solution. Non‐zero current measured at zero bias under illumination indicates that the process takes place. A degradation of the GaN structure is observed after a prolonged process time. In short‐term exposures, etching of microrod sidewalls is observed. Roughening of the a‐plane walls studied by transmission electron microscopy indicates that this orientation is etched with a fastest rate. The internal crystalline structure is not influenced by the etching and remains stable as shown by the X‐ray absorption spectroscopy study.

High-quality Ge/SiGe heterostructure with atomically sharp interface grown by molecular beam epitaxy

Germanium is a versatile material for realization of spin and topological quantum computing. Here, we report on the epitaxial growth of an undoped Ge/SiGe heterostructure in which a hole quantum well is formed in the sandwiched Ge layer. The heterostructure is grown on Si (001) via molecular beam epitaxy (MBE). Atomic force microscopy characterizations display a flat surface with a root mean square roughness of 0.956 nm, and spherical aberration corrected transmission electron microscopy data show a sharp interface with a characteristic length of 0.49 nm. A mobility of up to 1.2 × 105 cm2 V−1 s−1 was achieved in the SiGe/Ge/SiGe two-dimensional hole gas (2DHG). The low percolation density of 3.70 × 1010 cm−2, light effective mass of 0.079 m0 (where m0 is the free electron mass), and large effective g-factor of 9.5 were obtained. These results show the potential of MBE-grown Ge 2DHG for semiconductor quantum computing.

High-quality thickness-tunable InAs nanowire crosses grown by molecular-beam epitaxy

InAs nanowire crosses show great potential applications in detection and braiding of Majorana zero modes. Controlled growth of high-quality and diameter tunable InAs nanowire crosses is fundamental for these applications. However, it is still difficult to freely and conveniently adjust the diameter of the free-standing InAs nanowire crosses grown by the conventional growth methods. Here, we report a new technique to realize the growth of high-quality thickness-tunable InAs nanowire crosses by molecular-beam epitaxy. GaAs nanowire crosses were firstly grown on the Si (100) substrates spontaneously by merging the <111>-oriented GaAs nanowires. InAs nanowire crosses were then obtained by in situ growth of InAs shells on the facets of GaAs nanowire cross cores. Detailed scanning and transmission electron microscopic observations and energy dispersive spectrum analyses confirm that the InAs nanowire crosses grown by this manner have continuous and smooth morphology and they are high-quality zinc-blende crystals. More importantly, the InAs shell is grown with the vapor-solid growth mechanism and the thickness of the InAs nanowire crosses can be tuned by varying the InAs shell growth time. Our work provides a valuable method for the controlled growth of thickness-tunable semiconductor nanowire crosses.

Comparison of AlN/GaN heterojunctions grown by molecular beam epitaxy with Al and Ga assistance

Although conventional III-nitride molecular-beam-epitaxy growth theories indicate that high-quality AlN should be prepared in Al-assisted regimes, AlN/GaN heterojunctions grown in Ga-assisted regimes actually demonstrate superior performances. In this letter, we compared Al-assisted and Ga-assisted grown AlN/GaN heterojunctions and explored the underlying mechanisms. Aberration-corrected transmission electron microscope, energy dispersive spectrometer, and atomic force microscopy measurements indicate that the Al-assisted growth results in partly-relaxed AlN of high-density defects, deteriorating AlN/GaN interfaces, and surface morphology consisting of irregular and truncated atomic steps. The Ga-assisted growth produces high-quality pseudomorphic AlN with excellent AlN/GaN interfaces, surface morphology, and electrical properties. It is suggested that the better crystalline quality and higher performances of the Ga-assisted grown samples are attributed to a lower N subsurface diffusion barrier resulting from a higher energy of the fcc adsorption positions in the adlayer-enhanced-lateral-diffusion model and intense thermal motions of Ga adatoms. It helps to understand the kinetics of metal-adlayer-enhanced growth of AlN and AlN/GaN heterojunctions at atomic scale and optimize the growth processes. Meanwhile, it is demonstrated that amorphization and Al diffusion near the AlN surfaces occur due to Pt bombardment on highly tensile-strained AlN during focused-ion-beam fabrications. It implies that large strain in AlN/GaN heterojunctions might be an important issue to be considered for device reliability.

ScAlInN/GaN heterostructures grown by molecular beam epitaxy

Rare-earth (RE) elements doped III-nitride semiconductors have garnered attention for their potential in advanced high-frequency and high-power electronic applications. We report on the molecular beam epitaxy of quaternary alloy ScAlInN, which is an encouraging strategy to improve the heterointerface quality when grown at relatively low temperatures. Monocrystalline wurtzite phase and uniform domain structures are achieved in ScAlInN/GaN heterostructures, featuring atomically sharp interface. ScAlInN (the Sc content in the ScAlN fraction is 14%) films with lower In contents (less than 6%) are nearly lattice matched to GaN, exhibiting negligible in-plane strain, which are excellent barrier layer candidates for GaN high electron mobility transistors (HEMTs). Using a 15-nm-thick Sc0.13Al0.83In0.04N as a barrier layer in GaN HEMT, a two-dimensional electron gas density of 4.00 × 1013 cm−2 and a Hall mobility of 928 cm2/V s, with a corresponding sheet resistance of 169 Ω/□, have been achieved. This work underscores the potential of alloy engineering to adjust lattice parameters, bandgap, polarization, interfaces, and strain in emerging RE-III-nitrides, paving the way for their use in next-generation optoelectronic, electronic, acoustic, and ferroelectric applications.

Generation of GHz surface acoustic waves in (Sc,Al)N thin films grown on free-standing polycrystalline diamond wafers by plasma-assisted molecular beam epitaxy

Abstract Telecommunication of the next generation demands filters that can operate in the 10 GHz range with sufficient bandwidths. For surface-acoustic-wave (SAW) devices this prerequisite translates into high sound velocities and high piezoelectric couplings. Wurtzite AlN on diamond, which exploits the strong piezoelectricity of AlN with the very high SAW velocity of diamond, has been considered a promising platform. A significant boost (up to a factor of 4) of the piezoelectric response can be obtained by alloying AlN with Sc. Here, the main challenge lies in the synthesis of highly-oriented thin (Sc,Al)N films on diamond. In this work, we aim at establishing a platform for SAW devices using plasma-assisted molecular beam epitaxy for the deposition of Sc0.2Al0.8N on diamond. We investigate the structural properties related to SAW generation gearing towards applications at high frequencies. To this end, we prepare (Sc,Al)N thin films using plasma-assisted MBE on polished polycrystalline diamond wafers and demonstrate the efficient generation of SAW modes with frequencies up to 8 GHz. Systematic studies of the dependence of the SAW velocity and electromechanical coupling coefficient on the Sc0.2Al0.8N film thickness is presented for various SAW modes. Our result demonstrates the potential of this material combination for future application that requires large bandwidth in the ultra-high frequency range.&amp;#xD;

High-temperature Brown-Zak oscillations in graphene/hBN moiré field effect transistor fabricated using molecular beam epitaxy

Graphene placed on hexagonal boron nitride (hBN) has received significant interest due to its excellent electrical performance and physics phenomena, such as superlattice Dirac points. Direct molecular beam epitaxy growth of graphene on hBN offers an alternative fabrication route for hBN/graphene devices. Here, we investigate the electronic transport of moiré field effect transistors (FETs) in which the conducting channel is monolayer graphene grown on hexagonal boron nitride by high temperature molecular beam epitaxy (HT-MBE). Alignment between hBN and HT-MBE graphene crystal lattices gives rise to a moiré-fringed hexagonal superlattice pattern. Its electronic band structure takes the form of a “Hofstadter butterfly”. When a strong magnetic field B is applied perpendicular to the graphene layer, the electrical conductance displays magneto-oscillations, periodic in B−1, over a wide range of gate voltages and temperatures up to 350 K. We attribute this behaviour to the quantisation of electronic charge and magnetic flux within each unit cell of the superlattice, which gives rise to so-called Brown-Zak oscillations, previously reported only in high-mobility exfoliated graphene. Thus, this HT-MBE graphene/hBN heterostructure provides a platform for observation of room temperature quantum effects and device applications.

Effect of As4 beam equivalent pressure on the growth dynamics of InAs films grown at low temperature on graphene layers

The present study investigates the growth of InAs films at low temperature on graphene synthesized via molecular beam epitaxy, emphasizing the effect of As4 beam equivalent pressure (5.0 × 10⁻6 Torr (low) and 4.5 × 10⁻⁵ (high)) on the growth dynamics. X-ray diffraction, scanning electron microscopy, and atomic force microscopy, along with correlation functions, revealed that monitoring the As4 beam equivalent pressure affects the structural properties of polycrystalline InAs films grown on the graphene/Si layer. The film thickness (particle size) was found to be 172 ± 10 nm and 216 ± 10 nm (40 ± 2 nm and 42 ± 2 nm) for the InAs layers grown at low and high As4 beam equivalent pressure. The increase in the film thickness and particle size with increasing the As4 beam equivalent pressure is attributed to improved material availability and surface kinetics due to the large migration energy of As compared to In and hence the larger diffusion length of In. Conversely, decreasing As4 beam equivalent pressure raises the roughness scaling exponent and enlarges interface width (0.17 µm and 0.31 µm for films grown at high and low As4 beam equivalent pressure) and lateral correlation length, implying smoother surfaces due to larger particles. These insights are pivotal for fabricating advanced semiconductors, underscoring As4 beam equivalent pressure's role in optimizing InAs films for electronic and optoelectronic applications.

Review of the Properties of GaN, InN, and Their Alloys Obtained in Cubic Phase on MgO Substrates by Plasma-Enhanced Molecular Beam Epitaxy

Review of the Properties of GaN, InN, and Their Alloys Obtained in Cubic Phase on MgO Substrates by Plasma-Enhanced Molecular Beam Epitaxy

Growth Conditions and Interfacial Misfit Array in SnTe (111) Films Grown on InP (111)A Substrates by Molecular Beam Epitaxy.

Tin telluride (SnTe) is an IV-VI semiconductor with a topological crystalline insulator band structure, high thermoelectric performance, and in-plane ferroelectricity. Despite its many applications, there has been little work focused on understanding the growth mechanisms of SnTe thin films. In this manuscript, we investigate the molecular beam epitaxy synthesis of SnTe (111) thin films on InP (111)A substrates. We explore the effect of substrate temperature, Te/Sn flux ratio, and growth rate on the film quality. Using a substrate temperature of 340 °C, a Te/Sn flux ratio of 3, and a growth rate of 0.48 Å/s, fully coalesced and single crystalline SnTe (111) epitaxial layers with X-ray rocking curve full-width-at-half-maxima of 0.09° and root-mean-square surface roughness as low as 0.2 nm have been obtained. Despite the 7.5% lattice mismatch between the SnTe (111) film and the InP (111)A substrate, reciprocal space mapping indicates that the 15 nm SnTe layer is fully relaxed. We show that a periodic interfacial misfit (IMF) dislocation array forms at the SnTe/InP heterointerface, where each IMF dislocation is separated by 14 InP lattice sites/13 SnTe lattice sites, providing rapid strain relaxation and yielding the high quality SnTe layer. This is the first report of an IMF array forming in a rock-salt on zinc-blende material system and at an IV-VI on III-V heterointerface, and highlights the potential for SnTe as a buffer layer for epitaxial telluride film growth. This work represents an important milestone in enabling the heterointegration between IV-VI and III-V semiconductors to create multifunctional devices.

Barrier heights and strong fermi-level pinning at epitaxially grown ferromagnet/ZnO/metal Schottky Interfaces for opto-spintronics applications

Schottky contacts at the ferromagnet/ZnO interface are good candidates for the realization and control of several semiconductor emerging magnetic phenomena such spin injection and spin-controlled photonics. In this work, we demonstrate the epitaxial growth of single-phase and wurtzite-ZnO thin films on fcc Pt/Co0.30Pt0.70 (111) electrodes by molecular beam epitaxy technique. While the magnetic properties of the Pt/Co0.30Pt0.70 buffer remain unchanged after the ZnO growth, the electric measurements of back-to-back Schottky diodes reveal Schottky barrier heights at the metal/ZnO interfaces in the range of 590–690 meV using Cu, Pt and Co0.30Pt0.70 contacts. A pinning factor S and a charge neutrality level (CNL) ΦCNL of 0.08 and 4.94 eV, respectively, are obtained indicating a strong Fermi-level pining with a CNL level that lies 0.64 eV bellow the conductance band of ZnO semiconductor. These experimental findings indicate that Co0.30Pt0.70/ZnO interface follows the metal-induced gap states model and can open a pathway for the realization of opto-spintronics applications such spin-LEDs.

Centimeter-scale above room temperature ferromagnetic Fe3GaTe2 thin films by molecular beam epitaxy

Abstract Fe3GaTe2, as a layered ferromagnetic material, has a Curie temperature (T c ) higher than room temperature, making it the key material in the next generation of spintronic devices. To be used in practical devices, large-size and high-quality Fe3GaTe2 thin films need to be prepared. Here, the centimeter-scale thin film samples with high crystal quality and above room temperature ferromagnetism with strong perpendicular magnetic anisotropy (PMA) have been prepared by molecular beam epitaxy technology. Furthermore, the T c of the samples raises as the film thickness increases, and reaches 367 K when the film thickness is 60 nm. This study provides material foundations for the new generation of van der Waals spintronic devices and paves the way for the commercial application of Fe3GaTe2.

Monolayer-scale AlN/GaN digital alloys grown by plasma-assisted molecular beam epitaxy

The efficiency of usual AlGaN based deep ultraviolet light-emitting devices is still quite low. The difficulties are basically originated from the fundamental material properties of AlGaN. This work has adopted monolayer-scale (AlN)m/(GaN)n ordered digital alloys (DAs) as alternatives to AlGaN random alloys, m and n are the numbers of monolayers. X-ray diffraction scans have demonstrated clear satellite peaks, verifying good periodicity of AlN/GaN DAs grown by molecular beam epitaxy (MBE), and transmission electron microscopy results have revealed atomically sharp and smooth interfaces and quite precise m:n values agreeing well with designs. The electron densities of Si-doped (AlN)m/(GaN)n DAs with high equivalent Al compositions are significantly higher than those of conventional AlGaN:Si random alloys grown in the same MBE system. Si dopant ionization energies in DAs are only 2–5 meV, much lower than that for usual random alloys. The red shift of the light emission for DAs with thinner AlN barriers has suggested strong coupling between the GaN wells and thus formation of a miniband in a vertical direction. The results have demonstrated the potential of the (AlN)m/(GaN)n DAs as electronically functional alternatives for various device applications.

Epitaxial growth of single unit-cell superconducting β-Bi2Pd

Bismuth-based binary alloy β-Bi2Pd has recently been suggested as a connate topological superconductor with immense promise for Majorana zero modes. However, the epitaxial thin films down to the ultimate level of single unit-cell have been challenging. Here, we employed the state-of-the-art molecular beam epitaxy to prepare single unit-cell superconducting β-Bi2Pd films with lateral dimensions of hundreds of nanometers. Utilizing in situ scanning tunneling microscopy/spectroscopy, we uncover evidence of anisotropic superconductivity whose spectra are well fit by anisotropic s-wave gap functions and demonstrate that the epitaxial growth of β-Bi2Pd films relies substantially on the substrate temperature, flux ratio, growth rate, and coverage. The high-quality epitaxial films provide a promising platform to investigate the topological superconductivity at the two-dimensional limit.

High-Quality Single Crystalline Sc0.37Al0.63N Thin Films Enabled by Precise Tuning of III/N Atomic Flux Ratio during Molecular Beam Epitaxy

We attained wurtzite ScxAl1−xN (0.16 ≤ x ≤ 0.37) thin films by varying the Sc and Al fluxes at a fixed active nitrogen flux during plasma-assisted molecular beam epitaxy. Atomic fluxes of Sc and Al sources via measured Sc percentage in as-grown ScxAl1−xN thin films were derived as the feedback for precise determination of the ScxAl1−xN growth diagram. We identified an optimal III/N atomic flux ratio of 0.78 for smooth Sc0.18Al0.82N thin films. Further increasing the III/N ratio led to phase separation under N-rich conditions, validated by the observation of high-Sc-content hillocks with energy-dispersive X-ray spectroscopy mapping. At the fixed III/N ratio of 0.78, we found that phase separation with high-Al-content hillocks occurs for x &gt; 0.37, which is substantially lower than the thermodynamically dictated threshold Sc content of ~0.55 in wurtzite ScxAl1−xN. We postulate that these wurtzite-phase purity degradation scenarios are correlated with adatom diffusion and the competitive incorporation process of Sc and Al. Therefore, the ScxAl1−xN growth window is severely restricted by the adatom kinetics. We obtained single crystalline Sc0.37Al0.63N thin films with X-ray diffraction (002)/(102) ω rocking curve full-width at half-maximums of 2156 arcsec and 209 arcsec and surface roughness of 1.70 nm. Piezoelectric force microscopy probing of the Sc0.37Al0.63N epilayer validates unambiguous polarization flipping by 180°.

Enhanced transport anisotropy of Bi film through carrier mobility modulation controlled by calcium metal

Ca-doped Bi films were fabricated on the glass substrate using the molecular beam epitaxy (MBE). The systematic evolution for the preferred orientation, transport properties and surface morphology of Bi films were observed in the change of doping content. The measurement results show the adjustability of the preferred orientated surface morphology and Bi film carrier mobility. As the doping content increases, the mobility ratio four-fold and increases the anisotropy. Transport measurement simplifies the characteristic analysis of topological quantum materials. This work controls the material quantum property by doping Ca using MBE, which extends the potential application of quantum anomalous Hall effect-based devices.

Unconventional magnetoresistance and resistivity scaling in amorphous CoSi thin films

The resistivity scaling of Cu electrical interconnects represents a critical challenge in Si CMOS technology. As interconnect dimensions reach below 10 nm, Cu resistivity increases significantly due to surface scattering. Topological materials have been considered for application in ultra-scaled interconnects (below 5 nm), due to their topologically protected surface states that have reduced electron scattering. Recent theoretical work on the topological chiral semimetal CoSi suggests that this material could offer lower resistivity than Cu at dimensions smaller than 10 nm. Here we investigate the scaling trend of textured and amorphous CoSi thin films, deposited by molecular beam epitaxy in a thickness range between 2 and 82.5 nm. Contrary to predictions of standard resistivity models, we report here a reduction in resistivity for thin amorphous CoSi films, which is instead consistent with surface-dominated transport. Moreover, magnetotransport measurements reveal significant enhancement of the magnetoresistance in scaled films, highlighting the complex transport mechanisms present in these highly disordered films at thicknesses of a few nanometers.

High-Mobility Carriers in Epitaxial IrO2 Films Grown using Hybrid Molecular Beam Epitaxy.

Binary rutile oxides of 5d metals such as IrO2 stand out in comparison to their 3d and 4d counterparts due to limited experimental studies, despite rich predicted quantum phenomena. Here, we investigate the electrical transport properties of IrO2 by engineering epitaxial thin films grown using hybrid molecular beam epitaxy. Our findings reveal phonon-limited carrier transport and thickness-dependent anisotropic in-plane resistance in IrO2 (110) films, the latter suggesting a complex relationship between strain relaxation and orbital hybridization. Magnetotransport measurements reveal a previously unobserved nonlinear Hall effect. A two-carrier analysis of this effect shows the presence of minority carriers with mobility exceeding 3000 cm2/(V s) at 1.8 K. These results point toward emergent properties in 5d metal oxides that can be controlled using dimensionality and epitaxial strain.